Mass spectrometric investigation of chemical conversion processes in flow reactors

连续反应器中化学转化过程的质谱研究

• 批准号: 239921178
• 负责人: Professorin Dr. Tina Kasper
• 金额: --
• 依托单位: Lehrstuhl für Thermodynamik
• 依托单位国家: 德国
• 项目类别: Research Units
• 财政年份: 2013
• 资助国家: 德国
• 起止时间: 2012-12-31 至 2022-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/239921178?language=en
• 关键词: Mass; spectrometric; investigation; chemical; conversion; Mass; spectrometric; investigation; chemical; conversion

The main objective of work in the research unit is to investigate the use of engines as flexible chemical reactors. In processes, referred to here as polygeneration, the engines should simultaneously provide higher-value chemicals, heat, and mechanical work. The planned work is the continuation of research performed in the project GV1 of the research unit FOR 1993.GV1 focusses on the investigation of the fundamental kinetic processes underlying the chemical conversion processes. In the third phase of the project, the main objective of the investigations is to assess the influence of ozone as additive on the formation of interesting chemicals because it is expected that ozone already activates the conversion reactions at very low concentrations. Fuel-rich gas mixtures are investigated in two types of flow reactors at temperatures between T = 300 – 1200 K, and high pressure (1 – 20 bar) for different residence times. The gas composition at the outlet of the reactor is analyzed by mass spectrometry and gas chromatography. Desired chemical conversion processes are all reactions that can potentially be used to store chemical energy, e.g. dehydrogenations, steam reforming, or C-C-coupling reactions, and partial oxidations. Conditions that lead to the formation of interesting products are identified by analyzing the product gas composition as function of the process parameters pressure, temperature or the residence time. Concentration profiles as function of reactor temperature or residence time serve as validation data for the development and testing of the “PolyMech” reaction mechanism developed in the research unit 1993. The reaction mechanism serves as a means of information transfer to apply results from the fundamental investigations to the application – the co-production of work and chemicals in the motor.The work in the third phase of the project relies on the methods already successfully implemented in the first two project phases and established collaborations. In the third project phase, biogenic fuels and additives (biogas, ethanol, methanol and oxymethylene ethers) will be used in addition to methane and natural gas to expand the accessible spectrum of products. The most important scientific question is, however, how the use of ozone as additive affects the chemical conversion processes. Ozone decomposes already at low temperature into reactive radicals and can activate the conversion reactions in this way. Since, in contrast to other additives, it does not compete with the fuel for the available oxygen, it does not limit the conversions of the fuel. Based on these observations, it will be investigated to what extent ozone can be used to improve the product yields and the selectivities of oxygenated and non-oxygenated products. As a result of the investigations, a fundamental kinetic understanding of the reaction mechanisms of ozone is generated.

研究部门工作的主要目的是研究发动机作为柔性化学反应器的使用。在此处称为多代的过程中，发动机应简单地提供高价值化学物质，热量和机械工作。计划的工作是在1993年研究部门的项目GV1项目中进行的研究继续进行。GV1的重点是化学转化过程基础的基本动力学过程的投资。在项目的第三阶段中，投资的主要目的是评估臭氧作为对有趣化学物质形成的添加剂的影响，因为预计臭氧已经激活了非常低浓度的转化反应。在T = 300 - 1200 K之间的两种类型的流动反应器中，研究了富含燃料的气体混合物，在不同的住宿时间之间，高压（1-20 bar）的高压（1-20 bar）研究了。通过质谱和气相色谱法分析反应器出口处的气体成分。所需的化学转化过程都是所有反应，可能用于储存化学能的反应，例如脱氢，蒸汽重整或C-C偶联反应和部分氧化。通过分析产品气体组成作为过程参数压力，温度或停留时间的功能，可以确定导致引起有趣产物的形成的条件。 Concentration profiles as function of reactor temperature or residence time serve as validation data for the development and testing of the “PolyMech” reaction mechanism developed in the research unit 1993. The reaction mechanism serves as a means of information transfer to apply results from the fundamental investments to the application – the co-production of work and chemicals in the motor.The work in the third phase of the project relies on the methods already successfully implemented in the first two project phases and established collaborations.在第三个项目阶段，除甲烷和天然气外，还将使用二元燃料和添加剂（沼气，乙醇，甲基醚）来扩展产品的可用谱。但是，最重要的科学问题是，使用臭氧作为添加剂如何影响化学转化过程。臭氧已经在低温下分解为反应性自由基，并可以以这种方式激活转化反应。由于与其他添加剂相比，它与可用氧气的燃料没有竞争，因此不会限制燃料的转化。基于这些观察结果，将在多大程度上使用臭氧来提高产品产量和氧化和非氧化产物的选择性。由于投资，对臭氧反应机制的基本动力学理解得以产生。